# Showing papers in "Physical Review B in 1999"

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TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.

Abstract: The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Bl\"ochl's projector augmented wave (PAW) method is derived. It is shown that the total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addition, critical tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed core all electron methods. These tests include small molecules $({\mathrm{H}}_{2}{,\mathrm{}\mathrm{H}}_{2}{\mathrm{O},\mathrm{}\mathrm{Li}}_{2}{,\mathrm{}\mathrm{N}}_{2}{,\mathrm{}\mathrm{F}}_{2}{,\mathrm{}\mathrm{BF}}_{3}{,\mathrm{}\mathrm{SiF}}_{4})$ and several bulk systems (diamond, Si, V, Li, Ca, ${\mathrm{CaF}}_{2},$ Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.

57,691 citations

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TL;DR: In this paper, a simple formulation of a generalized gradient approximation for the exchange and correlation energy of electrons has been proposed by Perdew, Burke, and Ernzerhof (PBE), which improves the chemisorption energy of atoms and molecules on transition-metal surfaces.

Abstract: A simple formulation of a generalized gradient approximation for the exchange and correlation energy of electrons has been proposed by Perdew, Burke, and Ernzerhof (PBE) [Phys. Rev. Lett. 77, 3865 (1996)]. Subsequently Zhang and Yang [Phys. Rev. Lett. 80, 890 (1998)] have shown that a slight revision of the PBE functional systematically improves the atomization energies for a large database of small molecules. In the present work, we show that the Zhang and Yang functional (revPBE) also improves the chemisorption energetics of atoms and molecules on transition-metal surfaces. Our test systems comprise atomic and molecular adsorption of oxygen, CO, and NO on Ni(100), Ni(111), Rh(100), Pd(100), and Pd(111) surfaces. As the revPBE functional may locally violate the Lieb-Oxford criterion, we further develop an alternative revision of the PBE functional, RPBE, which gives the same improvement of the chemisorption energies as the revPBE functional at the same time as it fulfills the Lieb-Oxford criterion locally.

5,971 citations

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TL;DR: In this article, the crystal potential and density are represented as a lattice sum of local overlapping nonspherical contributions, and the decomposition of the exchange and correlation potential into local parts is done using a technique of partitioning of unity resulting in local shape functions, which add exactly to unity in the whole crystal.

Abstract: We present a full-potential band-structure scheme based on the linear combination of overlapping nonorthogonal orbitals. The crystal potential and density are represented as a lattice sum of local overlapping nonspherical contributions. The decomposition of the exchange and correlation potential into local parts is done using a technique of partitioning of unity resulting in local shape functions, which add exactly to unity in the whole crystal and which are very easily treated numerically. The method is all-electron, which means that core relaxation is properly taken into account. Nevertheless, the eigenvalue problem is reduced to the dimension of a minimum valence orbital basis only. Calculations on sp and transition metals give results comparable to other full-potential methods. The calculations on the diamond lattice demonstrate the applicability of our approach to open structures. The consequent local description of all real-space functions allows the treatment of substitutional disordered materials.

1,568 citations

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TL;DR: In this paper, a dipole correction that cancels the artificial electric field was proposed to study an asymmetric slab with a net surface dipole density, and the results were supported by total energy calculations of water-molecule layers.

Abstract: When performing density-functional calculations of surfaces using a plane-wave pseudopotential code, it is necessary to embed a slab with two surfaces in a periodic supercell. In many situations, it is desirable to study an asymmetric slab with a net surface dipole density. The periodic boundary conditions imposed on the electrostatic potential then give rise to an artificial electric field across the slab. We present a dipole correction that cancels the artificial field, and show how this correction can be incorporated in the density-functional theory total-energy expression. The results are supported by total-energy calculations of water-molecule layers.

1,444 citations

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TL;DR: In this article, an approach to the development of many-body interatomic potentials for monoatomic metals with improved accuracy and reliability is presented. But the functional form of the potentials is that of the embedded-atom method, but the interesting features are as follows: (1) the database used for the development a potential includes both experimental data and a large set of energies of different alternative crystalline structures of the material generated by ab initio calculations.

Abstract: We demonstrate an approach to the development of many-body interatomic potentials for monoatomic metals with improved accuracy and reliability. The functional form of the potentials is that of the embedded-atom method, but the interesting features are as follows: (1) The database used for the development of a potential includes both experimental data and a large set of energies of different alternative crystalline structures of the material generated by ab initio calculations. We introduce a rescaling of interatomic distances in an attempt to improve the compatibility between experimental and ab initio data. (2) The optimum parametrization of the potential for the given database is obtained by alternating the fitting and testing steps. The testing step includes a comparison between the ab initio structural energies and those predicted by the potential. This strategy allows us to achieve the best accuracy of fitting within the intrinsic limitations of the potential model. Using this approach we develop reliable interatomic potentials for Al and Ni. The potentials accurately reproduce basic equilibrium properties of these metals, the elastic constants, the phonon-dispersion curves, the vacancy formation and migration energies, the stacking fault energies, and the surface energies. They also predict the right relative stability of different alternative structures with coordination numbers ranging from 12 to 4. The potentials are expected to be easily transferable to different local environments encountered in atomistic simulations of lattice defects.

1,269 citations

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TL;DR: In this paper, a quantum-gate mechanism based on electron spins in coupled semiconductor quantum dots is considered and the magnetization and the spin susceptibilities of the coupled dots are calculated.

Abstract: We consider a quantum-gate mechanism based on electron spins in coupled semiconductor quantum dots. Such gates provide a general source of spin entanglement and can be used for quantum computers. We determine the exchange coupling $J$ in the effective Heisenberg model as a function of magnetic $(B)$ and electric fields, and of the interdot distance $a$ within the Heitler-London approximation of molecular physics. This result is refined by using $\mathrm{sp}$ hybridization, and by the Hund-Mulliken molecular-orbit approach, which leads to an extended Hubbard description for the two-dot system that shows a remarkable dependence on $B$ and $a$ due to the long-range Coulomb interaction. We find that the exchange $J$ changes sign at a finite field (leading to a pronounced jump in the magnetization) and then decays exponentially. The magnetization and the spin susceptibilities of the coupled dots are calculated. We show that the dephasing due to nuclear spins in GaAs can be strongly suppressed by dynamical nuclear-spin polarization and/or by magnetic fields.

1,178 citations

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TL;DR: In this paper, the magnetic properties of ribbon-shaped nanographite systems with zigzag and armchair edges in a magnetic field were investigated by using a tight-binding model.

Abstract: Electronic and magnetic properties of ribbon-shaped nanographite systems with zigzag and armchair edges in a magnetic field are investigated by using a tight-binding model. One of the most remarkable features of these systems is the appearance of edge states, strongly localized near zigzag edges. The edge state in a magnetic field, generating a rational fraction of the magnetic flux ( f5 p/q) in each hexagonal plaquette of the graphite plane, behaves like a zero-field edge state with q internal degrees of freedom. The orbital diamagnetic susceptibility strongly depends on the edge shapes. The reason is found in the analysis of the ring currents, which are very sensitive to the lattice topology near the edge. Moreover, the orbital diamagnetic susceptibility is scaled as a function of the temperature, Fermi energy, and ribbon width. Because the edge states lead to a sharp peak in the density of states at the Fermi level, the graphite ribbons with zigzag edges show Curie-like temperature dependence of the Pauli paramagnetic susceptibility. Hence, there is a crossover from hightemperature diamagnetic to low-temperature paramagnetic behavior in the magnetic susceptibility of nanographite ribbons with zigzag edges. @S0163-1829~99!02111-6#

1,116 citations

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TL;DR: In this article, the authors measured the temperature-dependent thermal conductivity of single-walled carbon nanotubes from 350 K to 8 K and showed that the thermal conductivities are dominated by phonons at all temperatures.

Abstract: We have measured the temperature-dependent thermal conductivity $\ensuremath{\kappa}(T)$ of crystalline ropes of single-walled carbon nanotubes from 350 K to 8 K. $\ensuremath{\kappa}(T)$ decreases smoothly with decreasing temperature, and displays linear temperature dependence below 30 K. Comparison with electrical conductivity experiments indicates that the room-temperature thermal conductivity of a single nanotube may be comparable to that of diamond or in-plane graphite, while the ratio of thermal to electrical conductance for a given sample indicates that the thermal conductivity is dominated by phonons at all temperatures. Below 30 K, the linear temperature dependence and estimated magnitude of $\ensuremath{\kappa}(T)$ imply an energy-independent phonon mean free path of \ensuremath{\sim}0.5--1.5 \ensuremath{\mu}m.

1,108 citations

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TL;DR: In this paper, the properties of two-dimensional periodic dielectric structures that have a band gap for propagation in a plane and that use index guiding to confine light in the third dimension are analyzed.

Abstract: We analyze the properties of two-dimensionally periodic dielectric structures that have a band gap for propagation in a plane and that use index guiding to confine light in the third dimension. Such structures are more amenable to fabrication than photonic crystals with full three-dimensional band gaps, but retain or approximate many of the latter's desirable properties. We show how traditional band-structure analysis can be adapted to slab systems in the context of several representative structures, and describe the unique features that arise in this framework compared to ordinary photonic crystals.

1,091 citations

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TL;DR: In this paper, a technique is presented to determine the spin statistics of excitons formed by electrical injection in a semiconducting organic thin film with the aid of selective addition of luminescent dyes.

Abstract: A technique is presented to determine the spin statistics of excitons formed by electrical injection in a semiconducting organic thin film. With the aid of selective addition of luminescent dyes, we generate either fluorescence or phosphorescence from the archetype organic host material aluminum tris (8-hydroxyquinoline) $({\mathrm{Alq}}_{3}).$ Spin statistics are calculated from the ratio of fluorescence to phosphorescence in the films under electrical excitation. After accounting for varying photoluminescent efficiencies, we find a singlet fraction of excitons in ${\mathrm{Alq}}_{3}$ of $(22\ifmmode\pm\else\textpm\fi{}3)%.$

1,004 citations

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TL;DR: In this article, the XPS core-and valence-level spectra of clean and well-characterized iron oxide films were analyzed and the satellite structures of each oxide were simulated using a cluster-model calculation.

Abstract: We report on a systematic analysis of x-ray photoelectron spectroscopy (XPS) core- and valence-level spectra of clean and well-characterized iron oxide films, i.e., $\ensuremath{\alpha}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3},$ $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3},$ ${\mathrm{Fe}}_{3\mathrm{\ensuremath{-}}\mathrm{\ensuremath{\delta}}}{\mathrm{O}}_{4},$ and ${\mathrm{Fe}}_{3}{\mathrm{O}}_{4}.$ All iron oxide films were prepared epitaxially by ${\mathrm{NO}}_{2}$-assisted molecular-beam epitaxy on single crystalline MgO(100) and $\ensuremath{\alpha}\ensuremath{-}{\mathrm{Al}}_{2}{\mathrm{O}}_{3}(0001)$ substrates. The phase and stoichiometry of the films were controlled precisely by adjusting the ${\mathrm{NO}}_{2}$ pressure during growth. The XPS spectrum of each oxide clearly showed satellite structures. These satellite structures were simulated using a cluster-model calculation, which could well reproduce the observed structures by considering the systematic changes in both the Fe $3d$ to O $2p$ hybridization and the $d\ensuremath{-}d$ electron-correlation energy. The small difference in the satellite structures between $\ensuremath{\alpha}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3}$ and $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3}$ resulted mainly from changes in the Fe-O hybridization parameters, suggesting an increased covalency in $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3}$ compared to $\ensuremath{\alpha}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3}.$ With increasing reduction in the $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{F}\mathrm{e}}_{3}{\mathrm{O}}_{4}$ system, the satellite structures in XPS became unresolved. This was not only due to the formation of ${\mathrm{Fe}}^{2+}$ ions, but also to nonhomogeneous changes in the hybridization parameters between octahedral and tetrahedral ${\mathrm{Fe}}^{3+}$ ions.

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TL;DR: In this paper, the elastic, electronic, and linear optical properties of quantum dot double heterostructures in the frame of eight-band quantum dot theory were investigated for a capped pyramid shaped InAs quantum dots in GaAs (001) with ${101}$ facets.

Abstract: We present a systematic investigation of the elastic, electronic, and linear optical properties of quantum dot double heterostructures in the frame of eight-band $\mathbf{k}\ensuremath{\cdot}\mathbf{p}$ theory. Numerical results for the model system of capped pyramid shaped InAs quantum dots in GaAs (001) with ${101}$ facets are presented. Electron and hole levels, dipole transition energies, oscillator strengths, and polarizations for both electron-hole and electron-electron transitions, as well as the exciton ground-state binding energy and the electron ground-state Coulomb charging energy are calculated. The dependence of all these properties on the dot size is investigated for base widths between 10 and $20$ nm. Results for two different approaches to model strain, continuum elasticity theory, and the Keatings valence force field model in the linearized version of Kane, are compared to each other.

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TL;DR: In this article, a database of surface segregation energies of single transition metal impurities in transition-metal hosts obtained by a Green's-function linear muffin-tin-orbitals method in conjunction with the coherent potential and atomic sphere approximations including a multipole correction to the electrostatic potential and energy is presented.

Abstract: We present a database of $24\ifmmode\times\else\texttimes\fi{}24$ surface segregation energies of single transition metal impurities in transition-metal hosts obtained by a Green's-function linear-muffin-tin-orbitals method in conjunction with the coherent potential and atomic sphere approximations including a multipole correction to the electrostatic potential and energy. We use the database to establish the major factors which govern surface segregation in transition metal alloys. We find that the calculated trends are well described by Friedel's rectangular state density model and that the few but significant deviations from the simple trends are caused by crystal structure effects.

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TL;DR: In this article, the structural, elastic, and vibrational properties of single-wall carbon nanotubes with different radii and chiralities were investigated using pseudopotential-density-functional theory, which allows calculations on systems with a large number of atoms per cell.

Abstract: A study based on ab initio calculations is presented on the structural, elastic, and vibrational properties of single-wall carbon nanotubes with different radii and chiralities. These properties are obtained using an implementation of pseudopotential-density-functional theory, which allows calculations on systems with a large number of atoms per cell. Different quantities are monitored versus tube radius. The validity of expectations based on graphite is explored down to small radii, where some deviations appear related to the curvature-induced rehybridization of the carbon orbitals. Young moduli are found to be very similar to graphite and do not exhibit a systematic variation with either the radius or the chirality. The Poisson ratio also retains graphitic values except for a possible slight reduction for small radii. It shows, however, chirality dependence. The behavior of characteristic phonon branches as the breathing mode, twistons, and high-frequency optic modes, is also studied, the latter displaying a small chirality dependence at the top of the band. The results are compared with the predictions of the simple zone-folding approximation. Except for the known deficiencies of the zone-folding procedure in the low-frequency vibrational regions, it offers quite accurate results, even for relatively small radii.

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TL;DR: In this article, the origin and dispersion of the anomalous disorder-induced Raman band (D$ band) observed in all hybridized disordered carbon materials near the K point of the Brillouin zone was investigated as a function of incident laser energy.

Abstract: The origin and dispersion of the anomalous disorder-induced Raman band $(D$ band) observed in all ${\mathrm{sp}}^{2}$ hybridized disordered carbon materials near 1350 ${\mathrm{cm}}^{\ensuremath{-}1}$ is investigated as a function of incident laser energy. This effect is explained in terms of the coupling between electrons and phonons with the same wave vector near the K point of the Brillouin zone. The high dispersion is ascribed to the coupling between the optic phonons associated with the D band and the transverse acoustic branch. The large Raman cross section is due to the breathing motion of these particular phonons near the K point. Our model challenges the idea that the Raman D peak is due to laser-energy-independent features in the phonon density of states, but rather is due to a resonant Raman process.

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TL;DR: Second-order nonlinear optics can be used to quantitatively determine the orientation of chemical bonds or submoieties of a fairly complicated molecule at an interface, and therefore completely map out its orientation and conformation as mentioned in this paper.

Abstract: Second-order nonlinear optics can be used to quantitatively determine the orientation of chemical bonds or submoieties of a fairly complicated molecule at an interface, and therefore completely map out its orientation and conformation. As a specific example, we have studied pentyl-cyanoterphenyl molecules at the air-water interface. We have measured the orientation of all three parts of the molecule (cyano head group, terphenyl ring, and pentyl chain) by optical second-harmonic generation and infrared-visible sum-frequency generation. A quantitatively consistent picture of the molecular configuration has been obtained. The technique can be applied to situations where other methods would fail (e.g., the surface of neat liquids or buried interfaces).

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TL;DR: In this paper, a unified theory for wave-packet dynamics of electrons in crystals subject to perturbations varying slowly in space and time is presented, where the wavepacket energy up to the first-order gradient correction and all kinds of Berry phase terms for the semiclassical dynamics and the quantization rule are derived.

Abstract: We present a unified theory for wave-packet dynamics of electrons in crystals subject to perturbations varying slowly in space and time. We derive the wave-packet energy up to the first-order gradient correction and obtain all kinds of Berry phase terms for the semiclassical dynamics and the quantization rule. For electromagnetic perturbations, we recover the orbital magnetization energy and the anomalous velocity purely within a single-band picture without invoking interband couplings. For deformations in crystals, besides a deformation potential, we obtain a Berry-phase term in the Lagrangian due to lattice tracking, which gives rise to new terms in the expressions for the wave-packet velocity and the semiclassical force. For multiple-valued displacement fields surrounding dislocations, this term manifests as a Berry phase, which we show to be proportional to the Burgers vector around each dislocation.

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TL;DR: In this paper, the Pfaffian quantum Hall states, which can be viewed as involving pairing either of spin-polarized electrons or of composite fermions, are generalized by finding the exact ground states of certain Hamiltonians with $k+1$-body interactions, for all integers $kg~1.

Abstract: The Pfaffian quantum Hall states, which can be viewed as involving pairing either of spin-polarized electrons or of composite fermions, are generalized by finding the exact ground states of certain Hamiltonians with $k+1$-body interactions, for all integers $kg~1.$ The remarkably simple wave functions of these states involve clusters of k particles, and are related to correlators of parafermion currents in two-dimensional conformal field theory. The $k=2$ case is the Pfaffian. For $kg~2,$ the quasiparticle excitations of these systems are expected to possess non-Abelian statistics, like those of the Pfaffian. For $k=3,$ these ground states have large overlaps with the ground states of the (two-body) Coulomb-interaction Hamiltonian for electrons in the first excited Landau level at total filling factors $\ensuremath{
u}=2+3/5,2+2/5.$

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TL;DR: In this paper, the authors describe a seamless coupling of continuum to statistical to quantum mechanics, involving an algorithm, implemented on a parallel computer, for handshaking between finite elements, molecular dynamics, and semi-empirical tight binding.

Abstract: A strategic objective of computational materials physics is the accurate description of specific materials on length scales approaching the meso and macroscopic. We report on progress towards this goal by describing a seamless coupling of continuum to statistical to quantum mechanics, involving an algorithm, implemented on a parallel computer, for handshaking between finite elements, molecular dynamics, and semiempirical tight binding. We illustrate and validate the methodology using the example of crack propagation in silicon.

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TL;DR: In this paper, femtosecond (fs) broadband transient absorption (TA) is used to study the intraband relaxation and depopulation dynamics of electron and hole quantized states in CdSe nanocrystals with a range of surface properties.

Abstract: Femtosecond (fs) broad-band transient absorption (TA) is used to study the intraband relaxation and depopulation dynamics of electron and hole quantized states in CdSe nanocrystals (NC's) with a range of surface properties. Instead of the drastic reduction in the energy relaxation rate expected due to a ``phonon bottleneck,'' we observe a fast subpicosecond $1P$-to-$1S$ electron relaxation, with the rate exceeding that due to phonon emission in bulk semiconductors. The energy relaxation is enhanced with reducing the NC's radius, and does not show any dependence on the NC surface properties (quality of the surface passivation). These data indicate that electron energy relaxation occurs by neither multiphonon emission nor by coupling to surface defects, but is likely meditated by Auger-type electron-hole energy transfer. We use fs infrared TA to probe electron and hole intraband transitions, which allows us to distinguish between electron and hole relaxation pathways leading to the depopulation of NC quantized states. In contrast to the electron relaxation, which is controlled by NC surface passivation, the depopulation of hole quantized states is extremely fast (sub-ps-to-ps time scales) in all types of samples, independent of NC surface treatment (including NC's overcoated with a ZnS layer). Our results indicate that ultrafast hole dynamics are not due to trapping at localized surface defects such as a vacancy, but rather arise from relaxation into intrinsic NC states or intrinsically unpassivated interface states.

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TL;DR: In this paper, a superconducting qubit that has circulating currents of opposite sign as its two states is presented. But the circuit consists of three nanoscale aluminum Josephson junctions connected in a super-conducting loop and controlled by magnetic fields.

Abstract: We present the design of a superconducting qubit that has circulating currents of opposite sign as its two states. The circuit consists of three nanoscale aluminum Josephson junctions connected in a superconducting loop and controlled by magnetic fields. The advantages of this qubit are that it can be made insensitive to background charges in the substrate, the flux in the two states can be detected with a superconducting quantum interference device, and the states can be manipulated with magnetic fields. Coupled systems of qubits are also discussed as well as sources of decoherence. @S0163-1829~99!00746-8#

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TL;DR: In this article, an atomic-scale simulation of the plastic behavior of nanocrystalline copper is presented, where the main deformation mode is sliding in the grain boundaries through a large number of uncorrelated events, where a few atoms (or tens of atoms) slide with respect to each other.

Abstract: Nanocrystalline metals, ie, metals in which the grain size is in the nanometer range, have a range of technologically interesting properties including increased hardness and yield strength We present atomic-scale simulations of the plastic behavior of nanocrystalline copper The simulations show that the main deformation mode is sliding in the grain boundaries through a large number of uncorrelated events, where a few atoms (or a few tens of atoms) slide with respect to each other Little dislocation activity is seen in the grain interiors The localization of the deformation to the grain boundaries leads to a hardening as the grain size is increased (reverse Hall-Petch effect), implying a maximum in hardness for a grain size above the ones studied here We investigate the effects of varying temperature, strain rate, and porosity, and discuss the relation to recent experiments At increasing temperatures the material becomes softer in both the plastic and elastic regime Porosity in the samples result in a softening of the material; this may be a significant effect in many experiments

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PARC

^{1}TL;DR: In this paper, the pseudopotential plane-wave method was used to perform density-functional calculations for III-V nitrides using the d states of the Ga and In atoms as valence states, and the results obtained using both the local density approximation (LDA) and the generalized gradient approximation (GGA) for the exchange-correlation functional are compared.

Abstract: We have performed density-functional calculations for III-V nitrides using the pseudopotential plane-wave method where the d states of the Ga and In atoms are included as valence states. Results obtained using both the local-density approximation (LDA) and the generalized gradient approximation (GGA) for the exchange-correlation functional are compared. Bulk properties, including lattice constants, bulk moduli and derivatives, cohesive energies, and band structures are reported for AlN, GaN, and InN in zinc-blende and wurtzite structures. We also report calculations for some of the bulk phases of the constituent elements. The performance of our pseudopotentials and various convergence tests are discussed. We find that the GGA yields improved physical properties for bulk Al, ${\mathrm{N}}_{2},$ and bulk AlN compared to the LDA. For GaN and InN, essentially no improvement is found: the LDA exhibits overbinding, but the GGA shows a tendency for underbinding. The degree of underbinding and the overestimate of the lattice constant as obtained within the GGA increases on going from GaN to InN. Band structures are found to be very similar within the LDA and GGA. For the III-V nitrides, the GGA therefore does not offer any significant advantages; in particular, no improvement is found with respect to the band-gap problem.

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TL;DR: In this paper, a method for atomic-scale modeling of the magnetic behavior of ionic magnetic solids is presented, where spin distributions and net magnetic moments are calculated for nanoparticles of ferrimagnetic and antiferromagnetic NiO as a function of applied field.

Abstract: We present a method for atomic-scale modeling of the magnetic behavior of ionic magnetic solids. Spin distributions and net magnetic moments are calculated for nanoparticles of ferrimagnetic ${\mathrm{NiFe}}_{2}{\mathrm{O}}_{4}$ and $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Fe}}_{2}{\mathrm{O}}_{3},$ and antiferromagnetic NiO as a function of applied field. Calculations incorporate crystal structures and exchange parameters determined from bulk data, bulk anisotropy for core spins, reasonable estimates for the anisotropy of surface spins, and finite temperatures simulated by random perturbations of spins. Surface spin disorder was found in the case of ferrimagnetic spinel nanoparticles, due to broken exchange bonds at the surface. The calculations also demonstrate that surface anisotropy enhances the coercivity of such particles only when surface spin disorder is present. Simulated thermal perturbations were used to characterize the distribution of energy barriers between surface spin states of such particles. The distribution of barriers can explain the macroscopic quantum tunneling like magnetic relaxation at low temperatures found experimentally. Calculations on NiO nanoparticles predict eight, six, or four-sublattice spin configurations in contrast to the two-sublattice configuration accepted for bulk NiO. Relatively weak coupling between the multiple sublattices allows a variety of reversal paths for the spins upon cycling the applied field, resulting in large coercivities and loop shifts, in qualitative agreement with experiment.

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TL;DR: In this article, a model of dispersive transport based on the continuous-time random walk is applied to nanocrystalline electrodes, where electrons perform a random walk on a lattice of trap states, each electron moving after a waiting time which is determined by the activation energy of the trap currently occupied.

Abstract: Electronic junctions made from porous, nanocrystalline ${\mathrm{TiO}}_{2}$ films in contact with an electrolyte are important for applications such as dye-sensitized solar cells. They exhibit anomalous electron transport properties: extremely slow, nonexponential current and charge recombination transients, and intensity-dependent response times. These features are attributed to a high density of intraband-gap trap states. Most available models of the electron transport are based on the diffusion equation and predict transient and intensity-dependent behavior which is not observed. In this paper, a preliminary model of dispersive transport based on the continuous-time random walk is applied to nanocrystalline ${\mathrm{TiO}}_{2}$ electrodes. Electrons perform a random walk on a lattice of trap states, each electron moving after a waiting time which is determined by the activation energy of the trap currently occupied. An exponential density of trap states $g(E)\ensuremath{\sim}{e}^{\ensuremath{\alpha}{(E}_{C}\ensuremath{-}E)/kT}$ is used giving rise to a power-law waiting-time distribution, $\ensuremath{\psi}{(t)=At}^{\ensuremath{-}1\ensuremath{-}\ensuremath{\alpha}}.$ Occupancy of traps is limited to simulate trap filling. The model predicts photocurrents that vary like ${t}^{\ensuremath{-}1\ensuremath{-}\ensuremath{\alpha}}$ at long time, and charge recombination transients that are approximately stretched exponential in form. Monte Carlo simulations of photocurrent and charge recombination transients reproduce many of the features that have been observed in practice. Using $\ensuremath{\alpha}=0.37,$ good quantitative agreement is obtained with measurements of charge recombination kinetics in dye-sensitized ${\mathrm{TiO}}_{2}$ electrodes under applied bias. The intensity dependence of photocurrent transients can be reproduced. It is also shown that normal diffusive transport, which is represented by $\ensuremath{\psi}(t)=\ensuremath{\lambda}{e}^{\ensuremath{-}\ensuremath{\lambda}t}$ fails to explain the observed kinetic behavior. The model is proposed as a starting point for a more refined microscopic treatment in which an experimentally determined density of states can be easily incorporated.

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TL;DR: In this article, the authors investigated the effect of tip sample separation, free amplitude, and sample properties on the performance of a force microscope with an amplitude modulation feedback, and showed that in the attractive regime, a net attractive force dominates the amplitude reduction while in the repulsive regime, amplitude reduction is dominated by a net repulsive force.

Abstract: Attractive and repulsive tip-sample interaction regimes of a force microscope operated with an amplitude modulation feedback were investigated as a function of tip-sample separation, free amplitude, and sample properties. In the attractive regime, a net attractive force dominates the amplitude reduction while in the repulsive regime the amplitude reduction is dominated by a net repulsive force. The transition between both regimes may be smooth or steplike, depending on free amplitude and sample properties. A steplike discontinuity is always a consequence of the existence of two oscillation states for the same conditions. Stiff materials and small free amplitudes give rise to steplike transitions while the use of large free amplitudes produce smooth transitions. Simulations performed on compliant samples showed cases where the cantilever dynamics is fully controlled by a net attractive force. Phase-shift measurements provide a practical method to determine the operating regime. Finally, we discuss the influence of those regimes in data acquisition and image interpretation.

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TL;DR: In this article, bisthiolterthiophene has been adsorbed on the two facing gold electrodes of a mechanically controllable break junction in order to form metal-molecule(s)-metal junctions.

Abstract: Molecules of bisthiolterthiophene have been adsorbed on the two facing gold electrodes of a mechanically controllable break junction in order to form metal-molecule(s)-metal junctions. Current-voltage $(I\ensuremath{-}V)$ characteristics have been recorded at room temperature. Zero bias conductances were measured in the 10--100 nS range and different kinds of nonlinear $I\ensuremath{-}V$ curves with steplike features were reproducibly obtained. Switching between different kinds of $I\ensuremath{-}V$ curves could be induced by varying the distance between the two metallic electrodes. The experimental results are discussed within the framework of tunneling transport models explicitly taking into account the discrete nature of the electronic spectrum of the molecule.

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TL;DR: In this paper, the authors studied the transport properties of pure and doped intermetallics of the form MNiSi (M=Zr, Hf), the structures known as the half-Heusler alloys.

Abstract: We have studied the transport properties in a family of pure and doped intermetallics of the form MNiSi (M=Zr, Hf), the structures known as the half-Heusler alloys. We have shown that the transport is very sensitive to structural arrangements of the constituent atoms, and this can be manipulated by annealing, isostructural alloying, and doping. The unusual transport properties are viewed in the context of a semimetal-semiconductor transition that in pure alloys sets in near 150 K. Doping with indium can shift the transition upward towards 200 K. The high-temperature transport is dominated by the presence of heavy electrons that are responsible for surprisingly large values of thermopower. Minute amount of antimony (n-type doping) have a spectacular influence on the nature of transport and drive the electrical resistivity and Hall effect to be metal-like at all temperatures. Sb-doped alloys display very high thermoelectric power factors, but the thermal conductivity is still too high to make the material a prospective thermoelectric.

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TL;DR: In this paper, surface reflectivity and emission spectra for multilayer dielectric waveguides with a two-dimensional patterning of deep holes are calculated using a scattering-matrix treatment to propagate electromagnetic waves through the structure.

Abstract: We present calculations of surface reflectivity and emission spectra for multilayer dielectric waveguides with a two-dimensional patterning of deep holes. The spectra are obtained using a scattering-matrix treatment to propagate electromagnetic waves through the structure. This treatment incorporates, in a natural way, the extended boundary conditions necessary to describe external reflection and emission processes. The calculated spectra demonstrate how such measurements can be used to obtain experimental information about the waveguide photonic band structure, the coupling of scattering modes to external fields, and the field distribution within the waveguide.

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TL;DR: In this paper, the emission and reflection spectra of ZnO have been investigated in the intrinsic region and the data have been interpreted in terms of the wurtzite crystal band structure.

Abstract: The emission and reflection spectra of ZnO have been investigated in the intrinsic region and the data have been interpreted in terms of the wurtzite crystal band structure. Free-exciton emission is observed for the first time. Both the ${\ensuremath{\Gamma}}_{5}$ and ${\ensuremath{\Gamma}}_{6}$ state excitons associated with top valence band have been identified. This identification has established the valence-band symmetry ordering in ZnO.